A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; Docherty, Kenneth S.; Jimenez, José L.

doi:10.5194/amt-9-5637-2016

Cited by 12 publications

(10 citation statements)

References 35 publications

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“…Despite this limitation, newly developed techniques for analyzing unresolved complex mixtures (UCM) may provide greater insight into trends in compounds and compound classes that would not otherwise be detectable. 51,52 This improved analysis will be the subject of future publications.…”

Section: Depletion Of Indoor Species Through Oxidationmentioning

confidence: 98%

Analysis of indoor particles and gases and their evolution with natural ventilation

et al. 2019

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Although people in developed nations spend up to 90% of their time indoors, 1,2 the chemistry and composition of indoor air remain understudied, especially compared to the outdoor environment. 3 Evaluating air quality in residential dwellings is particularly important for several reasons. First, although building standards (eg, for minimum air change rates and moisture control) have been established over the past several decades, 4,5 many residential structures fail to meet these standards, especially older buildings. Newer buildings, designed to minimize outdoor-to-indoor infiltration for improved energy efficiency, often have higher concentrations of airborne pollutants that are released indoors from materials and activities. 6,7 Concentrations and composition AbstractThe air composition and reactivity from outdoor and indoor mixing field campaign was conducted to investigate the impacts of natural ventilation (ie, window opening and closing) on indoor air quality. In this study, a thermal desorption aerosol gas chromatograph (TAG) obtained measurements of indoor particle-and gas-phase semi-and intermediately volatile organic compounds both inside and outside a single-family test home. Together with measurements from a suite of instruments, we use TAG data to evaluate changes in indoor particles and gases at three natural ventilation periods. Positive matrix factorization was performed on TAG and adsorbent tube data to explore five distinct chemical and physical processes occurring in the indoor environment. Outdoor-to-indoor transport is observed for sulfate, isoprene epoxydiols, polycyclic aromatic hydrocarbons, and heavy alkanes. Dilution of indoor species is observed for volatile, non-reactive species including methylcyclohexane and decamethylcyclopentasiloxane. Window opening drives enhanced emissions of semi-and intermediately volatile species including TXIB, DEET, diethyl phthalate, and carvone from indoor surfaces. Formation via enhanced oxidation was observed for nonanal and 2-decanone when outdoor oxidants entered the home. Finally, oxidative depletion of gas-phase terpenes (eg, limonene and α-pinene) was anticipated but not observed due to limited measurement resolution and dynamically changing conditions. K E Y W O R D Sfield measurements, gas chromatography-mass spectrometry, gas-particle partitioning, natural ventilation, residential air quality, semivolatile organic compounds

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Section: Depletion Of Indoor Species Through Oxidationmentioning

confidence: 98%

Analysis of indoor particles and gases and their evolution with natural ventilation

et al. 2019

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“…The shortcomings of low time resolution with filter measurements can be overcome using this kind of instruments to elucidate more information about the chemical processes involved. Such instrumentations include, for instance, TAG-AMS (thermal desorption aerosol gas chromatograph-AMS) [359][360][361], EESI-TOF-MS (extractive electrospray ionization-time of flight-MS) [362][363][364][365][366], or different inlets associated to PTR-MS (proton-transfer reaction-MS) or CIMS (chemical ionization MS) such as FIGAERO (filter inlet for gases and aerosols) [367], CHARON (chemical analysis of aerosol online) or thermo-desorption (TD) systems [37,[368][369][370][371], which have been successfully applied to apportion SOC in details. However, these instruments are still costly and only appropriate for short term studies.…”

Section: Conclusion and Future Implicationsmentioning

confidence: 99%

Comparison of Measurement-Based Methodologies to Apportion Secondary Organic Carbon (SOC) in PM2.5: A Review of Recent Studies

et al. 2018

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Secondary organic aerosol (SOA) is known to account for a major fraction of airborne particulate matter, with significant impacts on air quality and climate at the global scale. Despite the substantial amount of research studies achieved during these last decades, the source apportionment of the SOA fraction remains difficult due to the complexity of the physicochemical processes involved. The selection and use of appropriate approaches are a major challenge for the atmospheric science community. Several methodologies are nowadays available to perform quantitative and/or predictive assessments of the SOA amount and composition. This review summarizes the current knowledge on the most commonly used approaches to evaluate secondary organic carbon (SOC) contents: elemental carbon (EC) tracer method, chemical mass balance (CMB), SOA tracer method, radiocarbon (14C) measurement and positive matrix factorization (PMF). The principles, limitations, challenges and good practices of each of these methodologies are discussed in the present article. Based on a comprehensive—although not exhaustive—review of research papers published during the last decade (2006–2016), SOC estimates obtained using these methodologies are also summarized for different regions across the world. Conclusions of some studies which are directly comparing the performances of different methodologies are then specifically discussed. An overall picture of SOC contributions and concentrations obtained worldwide for urban sites under similar conditions (i.e., geographical and seasonal ones) is also proposed here. Finally, further needs to improve SOC apportionment methodologies are also identified and discussed.

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“…CC BY 4.0 License. retention time according to the method outlined in previous work (Zhang et al, 2014(Zhang et al, , 2016. Prior to chromatogram binning, each chromatogram was blank-subtracted to minimize the contribution of background noise in PMF calculations.…”

Section: Tag Positive Matrix Factorizationmentioning

confidence: 99%

“…First, the chemical composition of laboratory-110 generated BBOA was explored to identify molecular tracers from the leaf and heartwood of the American white oak (Quercus alba). Recently developed chromatogram-binning Positive Matrix Factorization (PMF) techniques (Zhang et al, 2014(Zhang et al, , 2016 were applied to the TAG compound window to determine the prevalence of different compound classes and functionalities unique to BBOA from each fuel type. Trends in compounds and compound classes of interest with oxidation were evaluated using both individual compound integrations and chromatogram binning PMF 115 results.…”

mentioning

confidence: 99%

“…These AMS parameters were used to inform interpretation of TAG decomposition ion signals, particularly the variation of TAG decomposition m/z 44 and m/z 60 signals with extent of oxidation in the PAM chamber. Additionally, 120 chromatogram-binning PMF techniques (Zhang et al, 2014(Zhang et al, , 2016 were applied to the decomposition window to investigate the presence and covariance of key ion signals. Finally, trends in TAG and AMS m/z 60 signals with PAM aging were explored to evaluate the utility of m/z 60 as a tracer for freshly-emitted BBOA.…”

mentioning

confidence: 99%

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Bulk and Molecular-Level Characterization of Laboratory-Aged Biomass Burning Organic Aerosol from Oak Leaf and Heartwood Fuels

Fortenberry¹,

Walker²,

Zhang³

et al. 2017

Preprint

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Abstract. The chemical complexity of biomass burning organic aerosol (BBOA) greatly increases with photochemical aging in the atmosphere, necessitating controlled laboratory studies to inform field observations. In these experiments, BBOA from American white oak (Quercus alba) leaf and heartwood samples was generated in a custom-built emissions and combustion chamber and photochemically aged in a Potential Aerosol Mass (PAM) flow reactor. A Thermal desorption Aerosol Gas chromatograph (TAG) was used in parallel with a high-resolution time-of-flight Aerosol Mass Spectrometer (AMS) to analyze BBOA chemical composition at different levels of photochemical aging. Individual compounds were identified and integrated to obtain relative decay rates for key molecular components. A recently-developed chromatogram binning positive matrix factorization (PMF) technique was used to obtain mass spectral profiles for factors in TAG BBOA chromatograms, improving analysis efficiency and providing a more complete determination of unresolved complex mixture (UCM) components. Additionally, the recently characterized TAG decomposition window was used to track molecular fragments created by the thermal decomposition of thermally labile BBOA during sample desorption. We demonstrate that while most components of primary BBOA decrease with photochemical aging, certain components eluting within the TAG thermal decomposition window instead increase. Specifically, the increasing trend in decomposition m&#8201;/&#8201;z 44 (CO2+) signals formation of secondary organic aerosol (SOA) in the PAM reactor. Sources of m&#8201;/&#8201;z 60 (C2H4O2+), typically attributed to freshly-emitted BBOA in AMS field measurements, were also investigated. From the TAG chemical speciation and decomposition window data, we observed a decrease in m&#8201;/&#8201;z 60 with photochemical aging due to the decay of anhydrosugars (including levoglucosan) and other compounds, as well as an increase in m&#8201;/&#8201;z 60 due to the formation of thermally labile organic acids within the PAM reactor, which decompose during TAG sample desorption. When aging both types of BBOA (leaf and wood), the AMS data exhibit a combination of these two contributing effects, causing limited change to the overall m&#8201;/&#8201;z 60 signal. Our observations demonstrate the importance of chemically-speciated data in fully understanding bulk aerosol measurements provided by the AMS in both laboratory and field studies.

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A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

Cited by 12 publications

References 35 publications

Analysis of indoor particles and gases and their evolution with natural ventilation

Analysis of indoor particles and gases and their evolution with natural ventilation

Comparison of Measurement-Based Methodologies to Apportion Secondary Organic Carbon (SOC) in PM2.5: A Review of Recent Studies

Bulk and Molecular-Level Characterization of Laboratory-Aged Biomass Burning Organic Aerosol from Oak Leaf and Heartwood Fuels

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